Hydrogen is a sustainable, clean, and affordable energy source which can used to generate more than three times of energy (149 MJ/kg) compared to petrol (48 MJ/kg). Also, water is produced as a byproduct. Water can be successfully converted to hydrogen via an integrated hydrogen evolution reaction (HER), which can then return to the same water molecule using solar radiation and continuous processing [1]. Also, hydrogen is toxic-free and can be converted into a material with high energy from renewable energy sources like water and light (photons) makes it a key component of the best energy for the future [2].

Since water currently makes up a bigger fraction of the cosmos, H2 is predominantly derived from one of the most abundant and renewable sources. To ensure economic growth, energy security, and environmental sustainability, Kondarides discussed three different sources in which we ultimately came to the conclusion that water was the best choice as our main source [3]. Hydrogen can be produced via photocatalytic water splitting approach and photocatalytic reforming of biomass (as illustrated in Fig. 1)

Fig 1: Three potential reaction pathways on the surface of the photocatalyst: biomass oxidation (right-hand reaction), photo-reforming (rectangular reaction), and water splitting (left-hand reaction) [3].

Photocatalysis is one of the highly studied processes that have the potential to yield a good outcome for hydrogen fuel production. Current advancements in steam reforming have increased hydrogen generation to 90% and necessitate the use of leftover fuel for CO2 adaption [4]. TiO2 photocatalyst produced in 1972 is unable to enhance Hydrogen production within the visible spectrum and it is imperative to find new methods that can do so [5,6]. This method must actively operate within the visible range and avoid the ultraviolet region to be efficient as a photocatalyst. As a result, numerous methods included to alter the band gap of TiO2, including the doping of metals and some non-metals between suitable semiconductors. Occasionally, the synthesis of ternary structured materials is used to achieve the desired band gap. Two additional techniques to narrow the band gap to 2.7 eV as a visible performance have been developed by Wen. Many studies have been conducted to obtain a profitable strategy to use copper oxide (CuO), reduced graphene (rGO), and Nickel ferrites (NiFe2O) to achieve a proficient solar conversion [7,8]. Besides, g-C3N4 could also be served as robust photocatalyst [9,10].

Splitting water into hydrogen could be one of the fascinating areas of study as it utilizes sunlight which is a sustainable energy source for chemical reactions. The reaction efficiency can still be enhanced selectivity towards desired products for improvement. In order to develop new photocatalysts with better characteristics (such as absorption of light and production of electron-hole pairs, engagement in redox reactions with other substances etc.) titanium dioxide must be enhanced with the capacity to split water into Hydrogen and Oxygen [11,12].

Fig 2: Schematic representation of redox reactions that take place on a photocatalyst after e-/h+ pairs are generated under light irradiation with energy higher than the Eg of the semiconductor. Water splitting (left-hand reactions) and oxidation (CxHyOz) under anaerobic conditions [12].

Semiconducting materials such as metal oxides (which include titanium dioxide or zinc oxide), and metal sulphides (cadmium and sulphide), or organic semiconductors (conjugated polymers) could be frequently used as photocatalysts. The energy difference between the conduction band (the lowest energy level available for electron excitation) and the valence band (which is the highest energy level occupied by electrons) is known as band gap of the materials. The valence band is left with positively charged holes when a photocatalyst absorbs photons with sufficient energy to excite electrons to the conduction band [12].

The process of the photocatalyst absorbing photons from the light source (often sunlight) is known as photon absorption. The absorbed photons excite electrons from the valence band to the conduction band, leaving behind positively charged holes in the valence band (the process is known as electron-hole generation). Excited electrons reduce water molecules to produce hydrogen gas (H2), whereas excited holes oxidize water to produce oxygen gas (O2) (redox reactions). During catalyst regeneration, the photocatalyst either receives electrons from an outside source or undergoes a reaction with sacrificial electron donors to return to its starting state [13].

The anodic processes that take place at one electrode and the cathodic reactions that happen at the other require a potential difference between them of more than 1.23 V for electrochemical breakdown of water. A radiation beam with a wavelength of 400-650nmis used to breakdown water with visible light.

One of the potential methods used for generating hydrogen is by using the combination of two different semiconductors as photocatalysts to absorb solar energy for water splitting process. This absorbed photons of light results in electron-hole pairs, in which the excited electrons could be oxidized and create holes while the holes convert protons (H+) into hydrogen gas (H2).The modified catalyst will lead the photocatalytic materials to absorb an abundant, and renewable solar energy of a wider spectrum of light for hydrogen production with the help of cocatalyst and sacrificial agent to speed up the reaction [13,14,15].

Fig 3: Reaction processes of water splitting on a catalyst photo catalyst [15].

Photo electrochemical (PEC) hydrogen production is another photocatalytic process of producing hydrogen gas, it is a combination of photo, electric and chemical materials together to obtain PEC semiconductor to generate hydrogen [16].

A fundamental (PC) and PEC can be considered as an effective hydrogen evolution reaction (HER) process. It results in the splitting of water into protons (h+) and electrons (e-) to generate hydrogen (H2) molecules.

                                                           (1.0)

The process can easily make electrons and protons to move back and forth for the efficient and targeted synthesis of hydrogen. It also serves as an environmentally friendly creation for high-purity hydrogen by noble metal catalysts, slow reaction kinetics, and simple catalytic activity and stability [17].

A collection of semiconductor materials that constitutes a crystal structure are known as perovskite minerals with a common formula ABX3. It is a cubic structure materials with A-site occupied by a large-size cation of organic (e.g. CH3NH3+, CH3CH2NH3+), inorganic, lanthanide metal (e.g. La, Ce, Pr, etc.) and alkaline (e.g. Ca, Sr, and Ba). The B-site is occupied by transition metals such as Co, Ru, Pb, Sn, Ge, etc. at body-center region. Cubic structured perovskites are categorized into three distinct groups of oxide perovskite, halide perovskite, and various perovskite as X-site, such variables can affect stability and flexibility of the structure in perovskite.

Fig 4: (a) ABX₃ perovskite unit cell, and (b) extended network structure of perovskites linked via the corner-shared octahedral [18].

Other perovskites exist which are called octahedrons with structural stability of the form BX. Many perovskites such as Titanates and Tantalates have band gap energies above visible range (i.e >3 eV) which hinders them from capturing majority of the solar spectrum. Band gap engineering is one of the greatest process of modifying Perovskites to improve charge separation, visible light absorption, and reduces recombination to obtain an efficient photocatalytic water splitting [19].

Photocatalyst needs to satisfy three fundamental requirements in order to obtain Hydrogen from water using visible light radiation and finally releases oxygen: (i) it ought to capture electron at the least photon of energy from 1.23 eV to 3.0 eV, this is equivalent 200-600 nm wavelength; and (ii) the conduction band (CB) potential required to be negative than redox potential (0 V vs NHE) (iii) valence band (VB) potential most be positive. Perovskites are among the materials that can offer such requirements with diverse advantages; such materials have suitable band edge potentials suitable for water splitting in hydrogen evolution reaction or the anodic oxygen evolution reaction with the help of band edge alignment. Secondly, perovskites have an adaptable nature of A and B sites cations structure loadings in various lattice arrangement which can be easily modified, thus enhancing many features for photocatalytic activity at unexceptional temperature and pressure such as magnetic and/or piezoelectric properties. Also, non-spontaneous water-splitting reactions results at the fluctuation stage close to Gibbs free energy of 237.3 kJ/mol [20].

Multiple perovskite photocatalysts have been developed and explore the ability of splitting water into Hydrogen, which includes binary or ternary compounds; such as nitride, metal oxide, phosphide, and sulphide for the development of a championship materials with suitable bandgap potential for the overall water splitting [21,22,23]. MTiO3 (M = Sr, Ba, Ca, Mn, Co, Fe, Pb, Cd, Ni); perovskites band gap has been modified from UV light to visible light absorption in order to be used as Photocatalytic or Photoelectrochemical materials for water splitting [21].

A-sites can be modified using band gap engineering by doping metal ions, while B-sites of BO6 could be replaced by anions dopants to change the majority of their band gap energy. While transition metals like (Cr, W, Fe, Ti, Ni, Mo, Ru, Rh, and others) could be doped ionically for enhancing the photocatalytic activity of single perovskites. Significant advancements have been achieved recently to customize single perovskite-based titanate oxides for photocatalytic HER [24,25].

Fig 5: H₂ evolution rate of several perovskite photocatalysts employing visible light irradiation in their bulk and Nano forms [25].

[39] Reported that SrTiO3, BaTiO3, MgTiO3, and ZnTiO3 are among the single perovskite-based titanate oxides with wide band gap energies of 3.0 eV and above that is achieved by modification of ionic dopant [26,27,10]. Fig. 6 shows the band gap and potentials of some titanate-based perovskites to split water.

Fig 6: Band gaps and edges of individual titanate-based perovskites in relation to the redox potential for splitting water [28].

CaTiO3 and MnTiO3 are two materials that can facilitate the production of Hydrogen in the presence of a trace amount of solar energy, while [97] reported thatSrTiO3 and CaTiO3 may insufficiently produce H2 under UV light irradiation. Doping or loading of the host materials would easily modify perovskite oxides and bring efficiently visible light absorption [3].

Titanate-Based Perovskite Photocatalysts

Many perovskites of different materials are considered for the application of photocatalytic hydrogen fuel generations; such as titanates, tantalates, ferrites and vanadate (see Fig. 7 showing the classification of perovskites), Among all of these, titanate-based perovskites serve as the most promising perovskites due to its excellent photostability, electronic properties, resistivity in a solution as well as the stability of photocatalytic activity under visible light [29]. These distinct properties attract interest to explore innovative ways of producing more effective materials by combining titanate and one of perovskite materials as a binary or ternary heterojunction structure at the same time doping new material to bring an effective result. This could be done when such materials are exposed to light, while photocatalyst absorbs photons and produces electron-hole pairs.

Fig 7: Classification of perovskite structures [30].

When titanate photocatalyst is developed, photogenerated electrons and holes could be engage in redox processes by splitting water molecules into hydrogen and oxygen with the help of band gap alignment. The band gap energy, light absorption, charge separation, and transfer efficiency may be improved by employing surface modification techniques, and heterojunction creation. The reduction of protons to hydrogen is frequently facilitated by the use of noble metal co-catalysts, such as platinum (Pt) or palladium (Pd), which enhances the catalytic performance [31,32,33,34,35].

Production of Visible Light Active Titanate-Based Perovskites

A strategic process is employed to synthesize titanate-based perovskite that entails the creation of the materials which are specifically ready for hydrogen production [35,36,30]. Any of the following methods of synthesis could be employed for both titanates and other perovskites, and non-perovskites materials to achieve the target: solid-state reactions, sol-gel procedures, hydrothermal synthesis, microwave absorption and Co-precipitate methods.

Table 1: Synthesis Methods for Perovskite Materials[30]

Out of six methods itemized on table 1; only Solid-state method presents a particle size with moderate agglomeration which present a low level of purity, while co-precipitate method has high prospects on both agglomeration and purity. Sol-gel also presents moderate but excellent materials in purity, auto combustion method brings low agglomeration but high purity. Microwave absorption and hydrothermal method gives low agglomeration at the same time have very high purity. Besides, hydrothermal method could be choosing as the best method of obtaining Nano particles as it can give more than hundred nanometer particle purity with low agglomeration.

Srtio3 Photocatalysts for Hydrogen Fuel Production

Strontium titanate can be improved to become a hybridize composite nanomaterial with reduced bandgap as photocatalytic hydrogen fuel source in order to satisfy its numerous advantages as a visible light absorbent [37]. Despite the advantages obtained by SrTiO3–based photocatalysts, variables such as high recombination and possibly instability could be controlled by adding foreign materials such as holes scavenger or co-catalyst [38,39,40].

Table 2: SrTiO₃-based material for Hydrogen (fuel) production via photo catalytic water splitting.

To easily produce hydrogen evolutions, pH levels are neutralized to the lowest ideal band structure, which result to highest amount of 491.5 µmol by using Pt as co-catalyst and TEOA as sacrificial agent when SrTiO3was synthesized via solvothermal method, while 347 mmol/h, 333 µmol/h, 200 µmol/h, 188µmol/hand 6.61mmol/h was obtained by using Au-Al, rGO/Pt, Au/Pt, Pt and Ag as co-catalysts respectively with methanol solution as shown in table 2.

Catio3 Photo catalytic Hydrogen Fuel Production

Band gap modification of CaTiO3-based composite could only be used to solve the larger band gap of calcium titanate in order to obtain highly effective photo catalytic material with low recombination and less photo-generated hole pair (since it is considered to be an inexpensive and low toxicity semiconductor) [46]. A hetero junction and co-catalyst materials can be used to overcome the challenges experience at the same time doping of metals and nonmetals [39,40,47].

Table3: CaTiO₃-based materials for Hydrogen (fuel) production via photo catalytic water splitting.

Many researchers have been conducted with CaTiO3 (Table 3) using the same method of synthesis (hydrothermal) in order to get hydrogen fuel production. Different quantities of hydrogen were obtained using different co-catalysts and sacrificial agents.

Zntio3 Photo catalytic Hydrogen Fuel Production

A hexagonal perovskite oxide material called Zinc titanate ZnTiO3 and some of its derivatives such as spinel (ZnTiO4), or defect spinel (ZnTiO8) Cubic Oxide perovskites are usually used for gas sensors, dielectric resonators and at times for oxidation and reduction of CO or NO. Coupling hexagonal perovskite and Titanium system reduces charge recombination as well as changing UV response to Visible light absorption for photo catalytic hydrogen fuel generation [56]. Also creating heterojunction with other materials will significantly increase the photo catalytic activity of ZnTiO3 [38,39,57].

Table 4: Active ZnTiO₃-based materials for Hydrogen (fuel) production via photocatalytic water splitting.

Cotio3 Photo catalytic Hydrogen Fuel Production

A nanostructured perovskite composite of Cobalt titanates (CoTiO3) are considered smart type catalyst that is potentially used for so many devices, like: magnetic recorders, gas sensors, and others. Heterogeneous photo catalysts may serve as important route to facilitate various reactions by importing new materials to significantly improve photo catalytic activity [38,39,61].

Table 5: Active CoTiO₃-based materials for Hydrogen (fuel) production via photo catalytic water splitting.

Cobalt titanate gives out small amount of hydrogen with the help of co-catalyst material and sacrificial agent. The result shows that without co-catalysts the promising component will not be obtained.

Nitio3 Photo Catalytic Hydrogen Fuel Production

Nickel titanate materials have attracted a lot of attention for solar fuel generation due to its unique properties such as inexpensive, low-toxicity, visible light absorption, suitable band gap of 3.0 eV, and photo stability to split water into hydrogen. Despite its unique properties, it also have defects such as low surface area and high recombination that needs to be overcome with some other processes [38,39,64,65].

Table 6: Active NiTiO₃-based materials for hydrogen (fuel) production via photo catalytic water splitting.

NiTiO3 gives exceedingly good results with the help of rGO, followed by CoS/CdS then TiO2 and CdS/CoS2 as co-catalysts while several sacrificial agents and methods are used.

Fetio3 Photo catalyst for Hydrogen Fuel Production

The greatest novelty for FeTiO3-based photo catalyst is oxygen evolution reaction, but researches make it useful for Hydrogen reaction by achieving fastest transfer of electrons in photo electrochemical reaction. Such efforts was done due to some of its properties which are: inexpensive, low-toxicity, photo stability and band gap of 2.8 eV [38,39,69,70].

Table 7: Active FeTiO₃-based materials for Hydrogen (fuel) production via photo catalytic water splitting.

There is paucity of research outcome on hydrogen due to its novelty on Oxygen evolution reaction.

Cdtio3 Photo catalytic Hydrogen Fuel Production

Most of the perovskite titanates considered as Titanium-based oxides with structural relation of MTiO3 (M = Cd, Ca, Ba, Sr, etc.) shows a distinct characteristic of electric and photo strictive materials similarities. Cadmium titanate (CdTiO3) is among such materials which is interestingly considered as photo catalytic titanates for hydrogen fuel production using visible light irradiation due to it special characteristic of 2.8 eV band gap as well as nice photo catalytic activity. Though, it is considered special; it does not make it the best as it have some drawbacks like high toxicity which contribute towards it less availability in literature [72].

Table 8: Active CdTiO₃-based materials for hydrogen (fuel) production via photo catalytic water splitting.

Pbtio₃ Photo catalytic Hydrogen Fuel Production

The photo catalytic efficiency of PbTiO3-based semiconductor is increased by introducing other perovskite substrates and syntheses through one of the best methods of syntheses to get a single domain nanomaterial that can adjust the band alignment of PbTiO3 photo catalytic hydrogen fuel production. Since it is among the best chosen semiconductor with suitable band gap of 2.7 eV, which is within visible light absorption, it negative part could easily been addressed by using sacrificial agents and some other methods [38,39,75,76].

Table 9: Active PbTiO₃-based materials for hydrogen (fuel) production via photo catalytic water splitting.

The unique properties of lead titanates has attracted interest in coupling PbTiO3 with other composite materials in order to have large amount of hydrogen but the yield has been relatively low (highest yield of 630.5 µmol/h) regardless of cocatalyst and sacrificial agents used.

Mntio3 Photo Catalytic Hydrogen Fuel Production

MnTiO3 perovskite-structured materials are widely used for oxygen carriers due to its bands location as they are all positive. Modifications done on its structure for the possibility of making it a visible light absorption material, controlling high recombination and obtaining hydrogen such as doping of metal oxides and other materials [38,39,82,83].

Batio3 Photo Catalytic Hydrogen Fuel Production

A-site of barium titanate (BaTiO3) containing larger ionic radii of Ba2+ with a structural perovskite of a bandgap at UV irradiation will be difficult to obtained hydrogen, but doping of another materials will adjust the bandgap to visible range for easy application of hydrogen production, its piezo and dielectric parameters could also be controlled [38,39,84,85]

Table 10: Active BaTiO₃-based materials for hydrogen (fuel) production via photo catalytic water splitting.

The highest amount of hydrogen obtained by BaTiO3 is789.7 µmol/g/h despites Pt and TEOA are used as cocatalyst and sacrificial agent, at the same time, single BaTiO3 is used with the help of TEOA by still gives out only 43.74 μmol/g/h of hydrogen.

General Discussion on Structural Adjustments of Perovskites for Hydrogen Production

A perovskite structure can be doped with a foreign element to engineer the photo catalyst electronic structures. This could be done with the combination of energies of the dopant and their host factors, the dopant can generate a new mid-gap state between the CB and VB or changes their position [90]. Doping a suitable element into the perovskite structure, the adjustment of band gap energy to the visible region could be achieved. For example,

SrTiO3 has a band gap of 3.2 eV, but when Rh is incorporated, the band gap is reduced, and leads to splitting water into H2 under the influence of visible light [91]. To control the band gap, Rh-doped at B-site component (Ti4+) energy of SrTiO3. Dopants can be obtained in both tetravalent (Rh4+) and trivalent ion (Rh3+) forms. For the purpose of being able to supply the charged electron to the SrTiO3 CB, Rh3+ provides a contributor level potential below at peak of the VB; as a result, the band gap may possibly become smaller. The energized electron transfer from the VB of SrTiO3 to newly created acceptor level as a result of Rh4+. As an alternative, Zn can be included into the A-site of SrTiO3 structure to control the band gap energy. This same process could be done to all perovskite for better action [92,93].

Table 11 outlines the most successful perovskite materials that have been engineered to generate reasonable amounts of hydrogen. These photo catalysts are fabricated by introducing foreign materials, starting from single perovskite oxides followed by doping single, double, and triple elements to main catalyst in order to bring higher generation of Hydrogen fuel.

Table 11: Titanate-based materials for hydrogen (fuel) production via photo catalytic water splitting [94].

Varying Morphologies and Crystal Structures of the Particles

The photo catalytic activity of perovskite photo catalysts is significantly impacted by the particle morphologies, along with crystal arrangement, particle size, and crystal structure. The photo excited charge separation and efficiency is one of the main challenges in developing effective photo catalysts for water splitting, this can easily be enhanced by altering particle morphologies of perovskite, even though this may not make them visible light active. Restructuring the perovskite photo catalysts' crystal structure can improve the photoelectron excitation and transfer process and increase photo catalytic activity.

Furthermore, due to the fact that defects such as grain boundaries (recombination sites) fewer and more common at high temperatures, high crystalline SrTiO3 show improved photo catalytic activity because, at high temperatures, calcination temperature increases with a decrease in the number of defects like grain boundaries (recombination sites) [105]. High calcination temperatures increase the photo catalyst crystallinity while boosting their particle size simultaneously. In addition, increased particle size can result in significant H2 evolution [105,106]. The rate of H2 production increase as the calcination temperature and crystallite size increases. High calcination temperatures boost H2 evolution by enhancing SrTiO3 crystallinity. In order to distinguish between crystallinity based on H2 evolution and the crystallite size effect, multiple SrTiO3 Nano fibers crystallite sizes were thus synthesized by varying the precursor concentrations at a constant calcination temperature.

Plasmonic Metal Addition

Incorporating plasmonic materials can drastically change all the Semiconductor properties (such as chemical and optical) because, the plasmonic resources exhibit a combined alternation of electrons in conduction that fluctuate at frequencies comparable to incidence of light [107]. Due to their strong capacity for stimulating catalytic processes, nanoparticles of Au and Ag have been frequently used visible light enhancement, and produce surface Plasmon resonance (SPR). Recently, Lu et al. synthesized a Nano porous single-crystalline SrTiO3 material with an Au surface modification for use in plasmonic photo catalysis. SrTiO3 is single-crystalline, thereby; mobility of induced SPR could enhance the photoelectrons. The surface area is highly providing for uniform scattering of Au particles, the optimized SPR-induced photoelectrons diffusion of the region more than polycrystalline SrTiO3 does. As a result, the fixed plasmonic Perovskite offers a different potential route by coming up with fresh ideas for designing water-splitting photo catalyst [108].

Heterojunction formation

Formation of heterostructure is a promising way to increase the performance of photo catalyst [9,109]. An appropriate heterojunction Nano-architecture can effectively separate the electron-hole pairs to absorb a large portion of the solar spectrum when electron-hole pairs are formed on semiconductor, then transmit to nearby materials [110,111]. Water splitting using SrTiO3 or NaTaO3 by themselves is impossible, however, both photo catalysts may split pure water when a heterostructure is formed using NiO [112,113]. To capture visible light stability, and improve charge separation, various research groups have begun to focus on the manufacture a heterojunction photo catalysts using appropriate band gap semiconductors.

Comprehensive light absorption is provided by low band gap semiconductors, although various band gap semiconductors become stable in aqueous solutions. Other titanate composites have been developed, particularly SrTiO3/Bi2O3, SrTiO3/CdS, SrTiO3/MoS2, and SrTiO3/Fe2O3 exhibits more effective activity than pure SrTiO3 as photo catalytic breakdown.

Recently, Wang et al., used the hybrid density functional of HSE06 to examine the geometry and electrical characteristics of SrTiO3/NaTaO3 heterostructures. The results of their study suggested that, compared to pure SrTiO3 and NaTaO3, SrTiO3/NaTaO3 heterostructures of each material having the narrow band gap of 2.58 eV, making them potential photocatalysts for visible light water splitting [114].

By conclusion; the review concentrated to make headway in perovskite-based material for efficient solar (H2) generation via PC water-splitting as follows:

• This review profound the methods of synthesis of titanate-Perovskites and adopted hydrothermal and co-precipitate as the most sustainable methods to actualize specific surface area, active surface sites, crystal structure, particle size and visible light absorption capacity.
• Integrate different titanates with other materials (such as; graphene, metal oxides, sulfides and phosphate) that can significantly enhance solar fuel (hydrogen) generation, thereby suppressing charge carrier recombination, creating active sites and extending visible light absorption, leading to higher activity.
• Perovskite materials, structural adjustment, method of synthesis, and Heterojunction mechanisms as well effect of sacrificial agents were fully discussed.

We acknowledged the support of the Department of Physics, Faculty of natural and applied science, Umaru Musa Yar’adua University (UMYU), Katsina-Nigeria. Umyu as an institution granted a permission under fellowship/leave to pursue my PhD Research at Federal University Dutse (FUD), Jigawa-Nigeria, I also acknowledged the support received from my supervisors for their words of encouragement, guidance, and commitments. This document has been produced and supposed financially by myself to achieve my PhD program as well development of my community and the entire world. The contents are the sole responsibility of the author(s).

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